Electrical transport, magnetic, and thermodynamic properties of La-, Pr-, and Nd-doped BaSn O3-δ single crystals

Eric McCalla, Daniel Phelan, Matthew J. Krogstad, Bogdan Dabrowski, Chris Leighton

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

Due to outstanding room temperature electron mobility, the wide-gap perovskite semiconductor BaSnO3 is of high current interest. Although n doping with Sb and O vacancies has been reported, most work has focused solely on La doping. Here we report bulk single crystals of Ba1-xRxSnO3-δ with R=La,Pr, and Nd, as well as unintentionally doped BaSnO3-δ, thus exploring new rare earth (magnetic) dopants in addition to O vacancy doping. Consistent with recent results on epitaxial films, O vacancies are shown capable of generating mid-1019cm-3 Hall electron densities, with single crystal mobilities ∼100-150cm2V-1s-1. Despite apparent solubility limits below ∼0.5at.%, Pr and Nd are also shown to be effective n dopants, yielding Hall electron densities >1×1020cm-3, and ambient and low temperature mobilities up to 175 and 430cm2V-1s-1, respectively. In contrast to the La-doped case, clear paramagnetism occurs with Pr and Nd doping, allowing for direct estimates of dopant concentrations for quantitative comparison with Hall densities. We show that dopant and Hall densities can be approximately reconciled, but only after accounting for O vacancy doping. Specific heat measurements were also performed, confirming the BaSnO3 Debye temperature, and revealing electronic contributions roughly consistent with reported effective masses. Interestingly, and likely related to crystalline electric field effects, Pr-doped BaSnO3 exhibits large deviations from simple Curie-Weiss susceptibility, and a pronounced Schottky anomaly, which we analyze in detail. These results provide significant insight into doping in BaSnO3, establishing new rare earth magnetic dopants, clarifying the role of O vacancies, and determining dopant concentrations and solubility limits.

Original languageEnglish (US)
Article number084601
JournalPhysical Review Materials
Volume2
Issue number8
DOIs
StatePublished - Aug 3 2018

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Transport properties
Magnetic properties
Thermodynamic properties
thermodynamic properties
transport properties
Doping (additives)
Single crystals
magnetic properties
single crystals
Vacancies
rare earth elements
solubility
specific heat
paramagnetism
electron mobility
Rare earths
ambient temperature
Carrier concentration
high current
heat measurement

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Electrical transport, magnetic, and thermodynamic properties of La-, Pr-, and Nd-doped BaSn O3-δ single crystals. / McCalla, Eric; Phelan, Daniel; Krogstad, Matthew J.; Dabrowski, Bogdan; Leighton, Chris.

In: Physical Review Materials, Vol. 2, No. 8, 084601, 03.08.2018.

Research output: Contribution to journalArticle

McCalla, Eric ; Phelan, Daniel ; Krogstad, Matthew J. ; Dabrowski, Bogdan ; Leighton, Chris. / Electrical transport, magnetic, and thermodynamic properties of La-, Pr-, and Nd-doped BaSn O3-δ single crystals. In: Physical Review Materials. 2018 ; Vol. 2, No. 8.
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AB - Due to outstanding room temperature electron mobility, the wide-gap perovskite semiconductor BaSnO3 is of high current interest. Although n doping with Sb and O vacancies has been reported, most work has focused solely on La doping. Here we report bulk single crystals of Ba1-xRxSnO3-δ with R=La,Pr, and Nd, as well as unintentionally doped BaSnO3-δ, thus exploring new rare earth (magnetic) dopants in addition to O vacancy doping. Consistent with recent results on epitaxial films, O vacancies are shown capable of generating mid-1019cm-3 Hall electron densities, with single crystal mobilities ∼100-150cm2V-1s-1. Despite apparent solubility limits below ∼0.5at.%, Pr and Nd are also shown to be effective n dopants, yielding Hall electron densities >1×1020cm-3, and ambient and low temperature mobilities up to 175 and 430cm2V-1s-1, respectively. In contrast to the La-doped case, clear paramagnetism occurs with Pr and Nd doping, allowing for direct estimates of dopant concentrations for quantitative comparison with Hall densities. We show that dopant and Hall densities can be approximately reconciled, but only after accounting for O vacancy doping. Specific heat measurements were also performed, confirming the BaSnO3 Debye temperature, and revealing electronic contributions roughly consistent with reported effective masses. Interestingly, and likely related to crystalline electric field effects, Pr-doped BaSnO3 exhibits large deviations from simple Curie-Weiss susceptibility, and a pronounced Schottky anomaly, which we analyze in detail. These results provide significant insight into doping in BaSnO3, establishing new rare earth magnetic dopants, clarifying the role of O vacancies, and determining dopant concentrations and solubility limits.

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